Steering Interzeolite Conversion with Alkali Metal Cations: Lithium Maximizes Al Proximity in SSZ-13 Zeolite Genesis

Sven Robijns, Julien Devos, Thibaut Donckels, Rodrigo de Oliveira-Silva, Niels De Witte, Dimitrios Sakellariou, Tom R. C. Van Assche, Michiel Dusselier

Research output: Contribution to journalArticlepeer-review

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Abstract

Zeolites have long been regarded as difficult to modify during synthesis, as their synthesis is governed by kinetic processes. Recent breakthroughs have made it possible to exert a certain degree of control over zeolite properties with more performant materials as a result. Here, we investigate the effects alkali cations have on high-silica FAU-toCHA interzeolite conversion (IZC) and on the resulting aluminum distributions. In this way, by using Li-cations in conjunction with an organic structure directing agent, the first route to a "fully paired" (divalent cation capacity, Co2+/Al = 0.48) high-silica SSZ-13 zeolite is demonstrated. Lithium shows great potential in steering IZC synthesis as it speeds up crystallization, and evidence was gathered in favor of a more elaborate mechanism of IZC in which dissolved Al-rich oligomers crash out of solution first and possibly spark nucleation. These findings help in gaining insights into a more general theory on zeolite nucleation in heterogeneous environments such as IZC. Furthermore, the "fully paired" sample has great potential for ion-exchanged zeolite catalysis or in adsorbents.
Original languageEnglish
Pages (from-to)289-299
Number of pages11
JournalCrystal Growth & Design
Volume23
Issue number1
Early online date22 Dec 2022
DOIs
Publication statusPublished - 4 Jan 2023

Bibliographical note

Funding Information:
S.R., N.D.W., T.R.C.V.A., and M.D. thank the Research Foundation─Flanders (FWO Vlaanderen) for funding (Grant G085220N). M.D. acknowledges funding from a Starting Grant from the European Research Council (ERC-2020-STG 948449, Z-EURECA). J.D. acknowledges KU Leuven for a PDM grant (3E210695) and Research Foundation─Flanders (FWO Vlaanderen) for funding (Grant 12E4623N). D.S. and R.O.-S. are grateful for the KU Leuven Starting Grant to D.S. and by the Research Foundation─Flanders (FWO Vlaanderen) under Grant PorMedNMR (G0D5419N) to D.S. SACHEM is explicitly thanked for providing the organic structure directing agent (TmAdamOH). The authors would also like to thank Prof. Jin Won Seo for her support for TEM imaging/troubleshooting and the Hercules Fund (Project AKUL/13/19) for financial support for the TEM.

Publisher Copyright:
© 2022 American Chemical Society.

Copyright:
Copyright 2023 Elsevier B.V., All rights reserved.

Keywords

  • cations
  • Crystallization
  • Oligomers
  • Solids
  • zeolites

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